Shaping the Water-Harvesting Behavior of Metal-Organic Frameworks Aided by Fine-Tuned GPT Models.

We construct a data set of metal-organic framework (MOF) linkers and employ a fine-tuned GPT assistant to propose MOF linker designs by mutating and modifying the existing linker structures. This strategy allows the GPT model to learn the intricate language of chemistry in molecular representations, thereby achieving an enhanced accuracy in generating linker structures compared with its base models. Aiming to highlight the significance of linker design strategies in advancing the discovery of water-harvesting MOFs, we conducted a systematic MOF variant expansion upon state-of-the-art MOF-303 utilizing a multidimensional approach that integrates linker extension with multivariate tuning strategies. We synthesized a series of isoreticular aluminum MOFs, termed Long-Arm MOFs (LAMOF-1 to LAMOF-10), featuring linkers that bear various combinations of heteroatoms in their five-membered ring moiety, replacing pyrazole with either thiophene, furan, or thiazole rings or a combination of two. Beyond their consistent and robust architecture, as demonstrated by permanent porosity and thermal stability, the LAMOF series offers a generalizable synthesis strategy. Importantly, these 10 LAMOFs establish new benchmarks for water uptake (up to 0.64 g g-1) and operational humidity ranges (between 13 and 53%), thereby expanding the diversity of water-harvesting MOFs.

ChatGPT Research Group for Optimizing the Crystallinity of MOFs and COFs.

We leveraged the power of ChatGPT and Bayesian optimization in the development of a multi-AI-driven system, backed by seven large language model-based assistants and equipped with machine learning algorithms, that seamlessly orchestrates a multitude of research aspects in a chemistry laboratory (termed the ChatGPT Research Group). Our approach accelerated the discovery of optimal microwave synthesis conditions, enhancing the crystallinity of MOF-321, MOF-322, and COF-323 and achieving the desired porosity and water capacity. In this system, human researchers gained assistance from these diverse AI collaborators, each with a unique role within the laboratory environment, spanning strategy planning, literature search, coding, robotic operation, labware design, safety inspection, and data analysis. Such a comprehensive approach enables a single researcher working in concert with AI to achieve productivity levels analogous to those of an entire traditional scientific team. Furthermore, by reducing human biases in screening experimental conditions and deftly balancing the exploration and exploitation of synthesis parameters, our Bayesian search approach precisely zeroed in on optimal synthesis conditions from a pool of 6 million within a significantly shortened time scale. This work serves as a compelling proof of concept for an AI-driven revolution in the chemistry laboratory, painting a future where AI becomes an efficient collaborator, liberating us from routine tasks to focus on pushing the boundaries of innovation.

A GPT-4 Reticular Chemist for Guiding MOF Discovery.

We present a new framework integrating the AI model GPT-4 into the iterative process of reticular chemistry experimentation, leveraging a cooperative workflow of interaction between AI and a human researcher. This GPT-4 Reticular Chemist is an integrated system composed of three phases. Each of these utilizes GPT-4 in various capacities, wherein GPT-4 provides detailed instructions for chemical experimentation and the human provides feedback on the experimental outcomes, including both success and failures, for the in-context learning of AI in the next iteration. This iterative human-AI interaction enabled GPT-4 to learn from the outcomes, much like an experienced chemist, by a prompt-learning strategy. Importantly, the system is based on natural language for both development and operation, eliminating the need for coding skills, and thus, make it accessible to all chemists. Our collaboration with GPT-4 Reticular Chemist guided the discovery of an isoreticular series of MOFs, with each synthesis fine-tuned through iterative feedback and expert suggestions. This workflow presents a potential for broader applications in scientific research by harnessing the capability of large language models like GPT-4 to enhance the feasibility and efficiency of research activities.

ChatGPT Chemistry Assistant for Text Mining and the Prediction of MOF Synthesis.

We use prompt engineering to guide ChatGPT in the automation of text mining of metal-organic framework (MOF) synthesis conditions from diverse formats and styles of the scientific literature. This effectively mitigates ChatGPT's tendency to hallucinate information, an issue that previously made the use of large language models (LLMs) in scientific fields challenging. Our approach involves the development of a workflow implementing three different processes for text mining, programmed by ChatGPT itself. All of them enable parsing, searching, filtering, classification, summarization, and data unification with different trade-offs among labor, speed, and accuracy. We deploy this system to extract 26 257 distinct synthesis parameters pertaining to approximately 800 MOFs sourced from peer-reviewed research articles. This process incorporates our ChemPrompt Engineering strategy to instruct ChatGPT in text mining, resulting in impressive precision, recall, and F1 scores of 90-99%. Furthermore, with the data set built by text mining, we constructed a machine-learning model with over 87% accuracy in predicting MOF experimental crystallization outcomes and preliminarily identifying important factors in MOF crystallization. We also developed a reliable data-grounded MOF chatbot to answer questions about chemical reactions and synthesis procedures. Given that the process of using ChatGPT reliably mines and tabulates diverse MOF synthesis information in a unified format while using only narrative language requiring no coding expertise, we anticipate that our ChatGPT Chemistry Assistant will be very useful across various other chemistry subdisciplines.

Estimating the total treatment effect in randomized experiments with unknown network structure.

Randomized experiments are widely used to estimate the causal effects of a proposed treatment in many areas of science, from medicine and healthcare to the physical and biological sciences, from the social sciences to engineering, and from public policy to the technology industry. Here we consider situations where classical methods for estimating the total treatment effect on a target population are considerably biased due to confounding network effects, i.e., the fact that the treatment of an individual may impact its neighbors' outcomes, an issue referred to as network interference or as nonindividualized treatment response. A key challenge in these situations is that the network is often unknown and difficult or costly to measure. We assume a potential outcomes model with heterogeneous additive network effects, encompassing a broad class of network interference sources, including spillover, peer effects, and contagion. First, we characterize the limitations in estimating the total treatment effect without knowledge of the network that drives interference. By contrast, we subsequently develop a simple estimator and efficient randomized design that outputs an unbiased estimate with low variance in situations where one is given access to average historical baseline measurements prior to the experiment. Our solution does not require knowledge of the underlying network structure, and it comes with statistical guarantees for a broad class of models. Due to their ease of interpretation and implementation, and their theoretical guarantees, we believe our results will have significant impact on the design of randomized experiments.

Unreasonable effectiveness of learning neural networks: From accessible states and robust ensembles to basic algorithmic schemes.

In artificial neural networks, learning from data is a computationally demanding task in which a large number of connection weights are iteratively tuned through stochastic-gradient-based heuristic processes over a cost function. It is not well understood how learning occurs in these systems, in particular how they avoid getting trapped in configurations with poor computational performance. Here, we study the difficult case of networks with discrete weights, where the optimization landscape is very rough even for simple architectures, and provide theoretical and numerical evidence of the existence of rare-but extremely dense and accessible-regions of configurations in the network weight space. We define a measure, the robust ensemble (RE), which suppresses trapping by isolated configurations and amplifies the role of these dense regions. We analytically compute the RE in some exactly solvable models and also provide a general algorithmic scheme that is straightforward to implement: define a cost function given by a sum of a finite number of replicas of the original cost function, with a constraint centering the replicas around a driving assignment. To illustrate this, we derive several powerful algorithms, ranging from Markov Chains to message passing to gradient descent processes, where the algorithms target the robust dense states, resulting in substantial improvements in performance. The weak dependence on the number of precision bits of the weights leads us to conjecture that very similar reasoning applies to more conventional neural networks. Analogous algorithmic schemes can also be applied to other optimization problems.

Emergence of tempered preferential attachment from optimization.

We show how preferential attachment can emerge in an optimization framework, resolving a long-standing theoretical controversy. We also show that the preferential attachment model so obtained has two novel features, saturation and viability, which have natural interpretations in the underlying network and lead to a power-law degree distribution with exponential cutoff. Moreover, we consider a generalized version of this preferential attachment model with independent saturation and viability, leading to a broader class of power laws again with exponential cutoff. We present a collection of empirical observations from social, biological, physical, and technological networks, for which such degree distributions give excellent fits. We suggest that, in general, optimization models that give rise to preferential attachment with saturation and viability effects form a good starting point for the analysis of many networks.